Ritobrata Sur

Analysis of calibration-free wavelength-scanned wavelength modulation spectroscopy for practical gas sensing using tunable diode lasers

A novel strategy has been developed for analysis of wavelength-scanned, wavelength modulation spectroscopy (WMS) with tunable diode lasers (TDLs). The method simulates WMS signals to compare with measurements to determine gas properties (e.g., temperature, pressure and concentration of the absorbing species). Injection-current-tuned TDLs have simultaneous wavelength and intensity variation, which severely complicates the Fourier expansion of the simulated WMS signal into harmonics of the modulation frequency (fm). The new method differs from previous WMS analysis strategies in two significant ways: (1) the measured laser intensity is used to simulate the transmitted laser intensity and (2) digital lock-in and low-pass filter software is used to expand both simulated and measured transmitted laser intensities into harmonics of the modulation frequency, WMS-nfm (n = 1, 2, 3,...), avoiding the need for an analytic model of intensity modulation or Fourier expansion of the simulated WMS harmonics. This analysis scheme is valid at any optical depth, modulation index, and at all values of scanned-laser wavelength. The method is demonstrated and validated with WMS of H2O dilute in air (1 atm, 296 K, near 1392 nm). WMS-nfm harmonics for n = 1 to 6 are extracted and the simulation and measurements are found in good agreement for the entire WMS lineshape. The use of 1f-normalization strategies to realize calibration-free wavelength-scanned WMS is also discussed.

Sensitive and rapid laser diagnostic for shock tube kinetics studies using cavity-enhanced absorption spectroscopy.

We report the first application of cavity-enhanced absorption spectroscopy (CEAS) using a coherent light source for sensitive and rapid gaseous species time-history measurements in a shock tube. Off-axis alignment and fast scanning of the laser wavelength were used to minimize coupling noise in a low-finesse cavity. An absorption gain factor of 83 with a measurement time resolution of 20 µs was demonstrated for C2H2 detection using a near-infrared transition near 1537 nm, corresponding to a noise-equivalent detection limit of 20 ppm at 296 K and 76 ppm at 906 K at 50 kHz. This substantial gain in signal, relative to conventional single-pass absorption, will enable ultra-sensitive species detection in shock tube kinetics studies, particularly useful for measurements of minor species and for studies of dilute reactive systems.

Time-resolved in situ detection of CO in a shock tube using cavity-enhanced absorption spectroscopy with a quantum-cascade laser near 4.6µm

Cavity-enhanced absorption spectroscopy (CEAS) using a mid-infrared DFB quantum-cascade laser is reported for sensitive time-resolved (10 μs) in situ CO measurements in a shock tube. Off-axis alignment and fast scanning of the laser wavelength were used to minimize coupling noise in a low-finesse cavity. An absorption gain factor of 91 was demonstrated, which enabled sub-ppm detection sensitivity for gas temperatures of 1000-2100K in a 15 cm diameter shock tube. This substantial improvement in detection sensitivity compared to conventional single-pass absorption measurements, shows great potential for the study of reaction pathways of high-temperature combustion kinetics mechanisms in shock tubes.

Line intensities and temperature-dependent line broadening coefficients of Q-branch transitions in the v2 band of ammonia near 10.4 μm

We report measured line intensities and temperature-dependent broadening coefficients of NH3 with Ar, N2, O2, CO2, H2O, and NH3 for nine sQ(J,K) transitions in the ν2 fundamental band in the frequency range 961.5-967.5 cm-1. This spectral region was chosen due to the strong NH3 absorption strength and lack of spectral interference from H2O and CO2 for laser-based sensing applications. Spectroscopic parameters were determined by multi-line fitting using Voigt lineshapes of absorption spectra measured with two quantum cascade lasers in thermodynamically-controlled optical cells. The temperature dependence of broadening was measured over a range of temperatures between 300 and 600 K. These measurements aid the development of mid-infrared NH3 sensors for a broad range of gas mixtures and at elevated temperatures.

Laser-absorption sensing of gas composition of products from coal gasification

A prototype in-situ laser-absorption sensor for the real-time composition measurement (CO, CH4, H2O and CO2) of synthesis gas products of coal gasification (called here syngas) was designed, tested in the laboratory, and demonstrated during field-measurement campaigns in a pilot-scale entrained flow gasifier at the University of Utah and in an engineering-scale, fluidized-bed transport gasifier at the National Carbon Capture Center (NCCC). The prototype design and operation were improved by the lessons learned from each field test. Laser-absorption measurements are problematic in syngas flows because efficient gasifiers operate at elevated pressures (10-50 atm) where absorption transitions are collision broadened and absorption transitions that are isolated at 1 atm become blended into complex features, and because syngas product streams can contain significant particulate, producing significant non-absorption scattering losses of the transmission of laser light. Thus, the prototype sensor used a new wavelength-scanned, wavelength-modulation spectroscopy strategy with 2f-detection and 1f-normalization (WMS-2f/1f) that can provide sensitive absorption measurements of species with spectra blended by collision broadening even in the presence of large non-absorption laser transmission losses (e.g., particulate scattering, beam steering, etc.). The design of the sensor for detection of CO, CH4, H2O and CO2 was optimized for the specific application of syngas monitoring at the output of large-scale gasifiers. Sensor strategies, results and lessons learned from these field measurement campaigns are discussed.